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If it's about the largest availability of books -- the answer is Amazon/Kindle if you live in the USA.
The eReader format is locked to a credit card number, so would allow you to use it on as many devices as you want -- but there are not yet any e-Ink devices that use the eReader format. ePub appears to require you to authorize through Adobe Digital Editions and I don't know exactly how it works with different devices, or changing computers, or reinstalling ADE. The DRM formats for LIT, Mobipocket, eReader, and ePub all appear to have been cracked, so you should be able to strip DRM to allow you to put the books onto any device you own.
Or hold out for non-DRMed books and buy only multi-fiction books from Fictionwise and Baen/Webscriptions.
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